Not sure what this is responding to, but excellent introduction to a really deep musical well! I would add to the Brazil list the stellar 1972 album Acabou Chorare by Novos Baianos, and note that Gilberto Gil's 1968 s/t album is, imo, the best album of the whole psychedelic period, and a great entry point (certainly more than the internationally famous Os Mutantes debut, which is great but significantly more experimental and less song-oriented - worth noting, too, that Os Mutantes are the backing band on Gilberto Gil 1968).

Otherwise, Jorge Ben made several great albums, the best of which are probably A Tábua de Esmeralda (1974) and África Brasil (1976). His mid-60's samba albums are also great fun (Samba Esquema Novo [1963] probably the most consistent).

Also, as a big fan of 1966-71 Chico Buarque, I'd caution that not understanding Portuguese takes more away from his work than any of the other artists mentioned, though it's probably still good even if jibberish to you.

Finally, can't leave out Elis & Tom (1974), quite possibly the best bossa nova album ever.

In Spanish, I'm not as knowledgeable, but Café Tacuba's Re (1994) is a definite must, esp. for anyone who likes themselves some Ween (i.e. shockingly consistent and well-done genre send-ups).